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51.
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Successive oxidation of transition metal(II) aqua complexes (M(II)OH(2) to M(III)OH) is a domain in which proton-coupled electron transfer reactions are extremely common. The mechanism of these PCET reactions-concerted or stepwise-is an important issue in the understanding and design of natural or artificial systems catalyzing the formation of dioxygen by four-electron oxidation of water. Concerted proton-coupled electron transfer from an aqua metal(II) to a hydroxo metal(III) complex requires the close proximity of a proton-accepting group with a pK value between those of the aqua complexes. Otherwise, stepwise electron-proton or proton-electron pathways involving high-energy intermediates are followed. Concerted proton-electron pathways involving water as proton-acceptor or proton-donor group are inefficient. Cyclic voltammetry of the title complex in buffered aqueous solution and re-examination of previous results for the same complex attached to an electrode surface are used to establish these conclusions, which provide a starting point on the route to higher degrees of oxidation, such as those involved in the catalysis of water oxidation. 相似文献
53.
J. Magan D. Lupo W. Praß U. Scheunemann P. Lemoine W. Blau M. Hogan 《Macromolecular Symposia》1991,46(1):253-257
Photoablation of several Langmuir-Blodgett (LB) films on Silicon substrates was performed at the excimer laser wavelength of 248 nm. This is a fast, solvent-free, one-step method for structuring thin organic films. Structures were produced both by projection of a mask and also using direct writing of the laser beam, yielding feature sizes on the order of microns. Spectral analysis of the remaining material showed no change compared to the unexposed material, suggesting that no degradation has occurred. This technique appears to be viable for use in the lithography of LB films. 相似文献
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Aitala EM Amato S Anjos JC Appel JA Ashery D Banerjee S Bediaga I Blaylock G Bracker SB Burchat PR Burnstein RA Carter T Carvalho HS Copty NK Costa I Cremaldi LM Darling C Denisenko K Fernandez A Gagnon P Gerzon S Gobel C Gounder K Halling AM Herrera G Hurvits G James C Kasper PA Kwan S Langs DC Leslie J Lundberg B MayTal-Beck S Meadows B de Mello Neto JR Milburn RH de Miranda JM Napier A Nguyen A d'Oliveira AB O'Shaughnessy K Peng KC Perera LP Purohit MV Quinn B Radeztsky S Rafatian A 《Physical review letters》1996,77(12):2384-2387
56.
Dr. David Teze Dr. Jiao Zhao Mathias Wiemann Dr. Zubaida G. A. Kazi Rossana Lupo Dr. Birgitte Zeuner Dr. Marlène Vuillemin Mette E. Rønne Dr. Göran Carlström Prof. Jens Ø. Duus Dr. Yves-Henri Sanejouand Dr. Michael J. O'Donohue Prof. Eva Nordberg Karlsson Dr. Régis Fauré Prof. Henrik Stålbrand Prof. Birte Svensson 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(40):10323-10334
Glycobiology is dogged by the relative scarcity of synthetic, defined oligosaccharides. Enzyme-catalysed glycosylation using glycoside hydrolases is feasible but is hampered by the innate hydrolytic activity of these enzymes. Protein engineering is useful to remedy this, but it usually requires prior structural knowledge of the target enzyme, and/or relies on extensive, time-consuming screening and analysis. Here, a straightforward strategy that involves rational rapid in silico analysis of protein sequences is described. The method pinpoints 6–12 single-mutant candidates to improve transglycosylation yields. Requiring very little prior knowledge of the target enzyme other than its sequence, the method is generic and procures catalysts for the formation of glycosidic bonds involving various d /l -, α/β-pyranosides or furanosides, and exo or endo action. Moreover, mutations validated in one enzyme can be transposed to others, even distantly related enzymes. 相似文献
57.
Stefania Sut Irene Ferrarese Maria Giovanna Lupo Nicola De Zordi Elisa Tripicchio Nicola Ferri Stefano Dall Acqua 《Molecules (Basel, Switzerland)》2021,26(13)
In the present study the ability of supercritical carbon dioxide (SCO2) extracts of M. longifolia L. leaves to modulate low-density lipoprotein receptor (LDLR) and proprotein convertase subtilisin/kexin type 9 (PCSK9) expression was evaluated in cultured human hepatoma cell lines Huh7 and HepG2. Two SCO2 extracts, one oil (ML-SCO2) and a semisolid (MW-SCO2), were subjected to detailed chemical characterization by mono- and bidimensional nuclear magnetic resonance (1D, 2D-NMR), gas chromatography coupled with mass spectrometry (GC-MS) and liquid chromatography coupled with mass spectrometry (LC-MS). Chemical analysis revealed significant amounts of fatty acids, phytosterols and terpenoids. ML-SCO2 was able to induce LDLR expression at a dose of 60 µg/mL in HuH7 and HepG2 cell lines. Furthermore, ML-SCO2 reduced PCSK9 secretion in a concentration-dependent manner in both cell lines. Piperitone oxide, the most abundant compound of the volatile constituent of ML-SCO2 (27% w/w), was isolated and tested for the same targets, showing a very effective reduction of PCSK9 expression. The overall results revealed the opportunity to obtain a new nutraceutical ingredient with a high amount of phytosterols and terpenoids using the SCO2 extraction of M. longifolia L., a very well-known botanical species used as food. Furthermore, for the first time we report the high activity of piperitone oxide in the reduction of PCSK9 expression. 相似文献
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Cunningham CH Chen AP Lustig M Hargreaves BA Lupo J Xu D Kurhanewicz J Hurd RE Pauly JM Nelson SJ Vigneron DB 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2008,193(1):139-146
Dynamic nuclear polarization and dissolution of a 13C-labeled substrate enables the dynamic imaging of cellular metabolism. Spectroscopic information is typically acquired, making the acquisition of dynamic volumetric data a challenge. To enable rapid volumetric imaging, a spectral-spatial excitation pulse was designed to excite a single line of the carbon spectrum. With only a single resonance present in the signal, an echo-planar readout trajectory could be used to resolve spatial information, giving full volume coverage of 32 × 32 × 16 voxels every 3.5 s. This high frame rate was used to measure the different lactate dynamics in different tissues in a normal rat model and a mouse model of prostate cancer. 相似文献
60.
Kowert BA Broeker GK Gentemann SJ Stemmler TL Fehr MJ Stemmler AJ Thurman-Keup EM McCoo PW Everett TB Lupo DJ Fitzsimmons PK Cordero AB 《The journal of physical chemistry. B》2007,111(47):13404-13409
The molecular motion of the planar bis(maleonitriledithiolato)nickel anion, Ni(mnt)(2)(-), has been studied as a function of temperature using electron spin resonance (ESR) in several polar solvents; they are ethyl alcohol, eugenol, dimethyl phthalate, tri-n-butyl phosphate, tris(2-ethyl-hexyl)phosphate, diglyme, and a dimethylformamide-chloroform mixed solvent. Calculated spectra in agreement with the experimental X-band spectra are obtained using axially symmetric reorientation when the long in-plane axis is the unique (parallel) axis of the rotational diffusion tensor with D parallel/D perpendicular = 3.0-4.0; D parallel and D perpendicular are the diffusion constants for reorientation about the parallel and perpendicular axes, respectively. The reorientational model required for the simulations is either in or close to the Brownian rotational diffusion limit. In the slow motional (low temperature) region, the spectra can be simulated using the glassy g values. As the temperature increases, however, agreement is obtained only if the intermediate g factor, g(y), for the non-axially symmetric Zeeman interaction increases while g(x), g(z), and the motional model remain unchanged; this scheme and others for which gx and g(z) are possibly temperature-dependent are discussed. The values of D perpendicular from the simulations are in general agreement with those from earlier analyses of the width of the central spectral feature. The simulations and width analyses indicate (as do electrochemical, conductivity, and vapor-phase osmometry data) that the paramagnetic species reorienting in solution has a shape similar to that of the Ni(mnt)(2)(-) ion. 相似文献